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Strain-Induced Lithium Losses in the Solid Electrolyte Interphase on Silicon Electrodes.

Ravi Kumar¹, Peng Lu², Xingcheng Xiao²

¹School of Engineering, Brown University , 182 Hope Street, Box D, Providence, Rhode Island 02912, United States.

ACS Applied Materials & Interfaces

|August 4, 2017

Summary

Strain in solid electrolyte interphase (SEI) layers significantly increases lithium consumption and inorganic phase formation. This study investigates SEI evolution under controlled strain, crucial for silicon anodes in high-capacity batteries.

Keywords:

capacity loss in situ atomic force microscope lithium-ion battery silicon anode solid electrolyte interphase

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Area of Science:

Materials Science
Electrochemistry
Battery Technology

Background:

Solid electrolyte interphase (SEI) layers are critical for the stability of high-capacity anode materials like silicon.
Silicon anodes experience substantial volume changes (~300%) during battery cycling, challenging SEI layer integrity.
Understanding SEI evolution under mechanical strain is key to improving battery performance and lifespan.

Purpose of the Study:

To investigate the impact of controlled mechanical strain on SEI formation and evolution in silicon electrodes.
To correlate irreversible capacity losses with SEI changes during silicon anode volume expansion and contraction.
To quantify lithium consumption and inorganic phase formation within the SEI layer under varying strain conditions.

Main Methods:

Development of a novel approach using patterned silicon electrodes to apply controlled strains to SEI films.
In situ Atomic Force Microscopy (AFM) combined with electrochemical measurements to monitor SEI growth and lithium loss.
Electrochemical Impedance Spectroscopy (EIS) and Time-of-Flight Secondary Ion Mass Spectrometry (TOF-SIMS) for detailed SEI characterization.

Main Results:

In-plane strain in the SEI layer directly correlates with increased lithium consumption.
Strain promotes substantial increases in inorganic phase formation within the SEI without significantly altering its overall thickness.
A comprehensive map of irreversible capacity evolution as a function of SEI strain was experimentally derived.

Conclusions:

Mechanical strain is a critical factor influencing SEI stability and lithium consumption in silicon anodes.
Controlled strain engineering of SEI layers can provide insights into battery degradation mechanisms.
The findings offer a pathway to optimize SEI properties for enhanced performance in next-generation high-capacity batteries.